【作者】 陈涛；

【导师】 晋冠平；

【作者基本信息】 合肥工业大学 ， 化学工程与技术， 2019， 硕士

【摘要】 通过电化学介导原子转移自由基法（eATRP）,在碳纤维上（CFs）接枝了2D结构的聚甲基丙烯酸缩水甘油酯前驱膜,并在其上原位修饰L-天冬氨酸,形成了3D结构的螯合碳纤维复合物（CCFs）;其后,依次原位电沉积镍铝层状复合金属氢氧化物（Ni/Al-LDHs）和亚铁氰化镍（NiHCF）,形成了可用于回收水溶性铯（Cs⁺）的功能性复合材料（NiHCF/NiAl-LDHs/CCFs）。采用电化学、FT-IR、XRD、SEM等技术对材料进行了表征。结果证明:CCFs具有3D结构,其上的Ni/Al-LDHs为多孔花状结构,NiHCF则嵌入在Ni/Al-LDHs层中。考察了NiHCF/NiAl-LDHs/CCFs在静态吸附法下对水溶液中Cs⁺的提取性能。在最佳条件下（pH 6,45℃,12 h）,NiHCF/NiAl-LDHs/CCFs对Cs⁺的最大吸附量为42.69 mg/g。采用两步分开的无膜的电化学开关离子交换法（MF-II-ESIX）,研究了NiHCF/NiAl-LDHs/CCFs对水溶液中Cs⁺的回收机制。在ESIX吸附过程中,在最佳条件下（pH 6,-0.4 V,4 h）,NiHCF/NiAl-LDHs/CCFs对Cs⁺的最大吸附容量为41.87 mg/g,相比于静态吸附法,其吸附时间缩短2/3,效率显著提高。解吸过程中,在最佳条件下（pH 7,-0.1¹.2 V,循环伏安120圈）,通过XPS表征发现:Cs⁺从NiHCF/NiAl-LDHs/CCFs-Cs⁺上的解吸效率可达85%以上,表明NiHCF/NiAl-LDHs/CCFs可以再生和重复使用。在最佳条件下,NiHCF/NiAl-LDHs/CCFs可用于盐湖卤水中Cs⁺的资源化回收。亚铁氰化铋改性石墨烯涂覆碳纤维复合材料（BiHCF/GN/CFs）,同时制备为多功能空气扩散电极和非均相光电Fenton催化剂,其中BiHCF用作Fe²⁺源和光催化剂代替经典Fenton中的铁盐溶液。通过SEM,XRD,FT-IR和电化学方法表征BiHCF/GN/CFs的形成。在光电Fenton过程中,以甲基橙为模型污染物,研究了BiHCF/GN/CFs对羟基自由基（?OH）的光电催化作用。由于优异的异相光电催化剂,光电Fenton工艺被用于甲基橙的有效降解,其中?OH可以在BiHCF/GN/CFs上,可见光照射下,-0.5^-0.9V电位范围内,通过O₂还原高效的光电产生。受益于BiHCF/GN/CFs的高?OH产率（4.88¹0.34 mM/h）,甲基橙（200mg/L）可在pH 4时以5.538⁶.29 h^-1的一级动力学常数快速降解,在35 min内甲基橙的去除率即可达到95%。更多还原

【Abstract】 2D-structured polyglycidyl methacrylate precursor film was grafted at surface of carbon fibers（CFs）by electrochemically mediated atom transfer radical method（eATRP）,and L-aspartic acid was modified in situ to form 3D structure of chelating carbon fiber composites（CCFs）;Ni-Al layered double hydroxides（Ni/Al-LDHs）and nickel hexacyanoferrates（NiHCF）were sequentially deposited in situ with the formation of NiHCF/NiAl-LDHs/CCFs,which was used to recover Cs⁺in aqueous solution.NiHCF/NiAl-LDHs/CCFs were characterized by FT-IR,XRD,SEM and electrochemical techniques.The CCFs displayed 3D structure,the Ni/Al-LDHs showed porous flower-like structures,and the NiHCF are embedded in the layer of the Ni/Al-LDHs.The uptake of NiHCF/NiAl-LDHs/CCFs towards Cs⁺in aqueous solution was investigated by static adsorption method.Under the optimal conditions（pH 6,45°C,12 h）,the maximum adsorption capacity was 42.69 mg/g.The recovery mechanism of NiHCF/NiAl-LDHs/CCFs towards Cs⁺in aqueous solution was studied during two-step membrane-free electrochemically switched ion exchange processes（ESIX）.In the adsorption process,under the optimal conditions（pH 6,-0.4 V,4 h）,the maximum adsorption capacity was 41.87 mg/g,the adsorption time was shortened 2/3 compared to that of static adsorption method with a significant efficiency.In the desorption process,under the optimal conditions（pH 7,-0.1¹.2 V,120 cycles）,85%of Cs⁺could be desorbed from the NiHCF/NiAl-LDHs/CCFs-Cs⁺by XPS analysis,the electrodes could be regenerated conveniently.Under the optimal conditions,NiHCF/NiAl-LDHs/CCFs could be used to the recovery of Cs⁺from salt lake brine.Bismuth hexacyanoferrate-modified graphene coated carbon fibers composite（BiHCF/GN/CFs）was prepared simultaneously as a multifunctional air diffusion electrode and heterogeneous photo-electro-Fenton catalyst,in which the BiHCF was used as the source of Fe²⁺and photo catalyst instead of a solution iron salt in classical Fenton.The formation of BiHCF/GN/CFs was characterized by SEM,XRD,FT-IR and electrochemical methods.The photo-electro catalysis of BiHCF/GN/CFs towards hydroxyl radical（?OH）was investigated during photo-electro-Fenton process with methyl orange（MO）as a model pollutant.Because of the excellent heterogeneous photo-electro-catalyst,the photo-electro-Fenton process was used for the efficient degradation of MO,where?OH could be vigorously photo-electro-generated from O₂ reduction at BiHCF/GN/CFs in a potential range of-0.5^-0.9 V under visible light.Benefited from the high?OH generating rate（4.88¹0.34 mM/h）at BiHCF/GN/CFs,MO（200 mg/L）could be rapidly degraded with first-order kinetic constants of 5.538⁶.29 h^-1 at pH 4,0.1 M Na₂SO₄,and the removal of MO was achieved to 95%within 35 min.更多还原